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DOE OSTI2024

Migration of 60 Co, 133 Ba, 137 Cs, and 152 Eu from cementitious wasteforms in field lysimeter experiments

Safe and effective storage of radioactive waste is essential to protect environmental health. Due to the potential for accidental releases and the severity of the associated risks, it is imperative to further understand radionuclide transport should an accident occur. This work analyzed the vadose zone migration of radionuclides from cementitious wasteforms at the Savannah River Site after ten years. The observed radionuclides are prominent constituents of radioactive waste or analogs for other groups or series of radionuclides. Lysimeters were first analyzed in 2016 using a collimated high-purity germanium gamma-ray spectrometer to non-destructively measure the concentration of each radionuclide in the sediment column as a function of depth. Following these measurements, the lysimeters were redeployed in the field for another 4 years. All radionuclides in all lysimeters were observed to transport further during the redeployment period; however, the extent of migration varied with the material used for introduction. Except for 137 Cs, migration through the sediment control system increased with decreasing ionic potential (ionic charge/radius); migration order: 152 Eu< 137 Cs< 60 Co< 133 Ba. Overall, the cementitious wasteforms were observed to decrease radionuclide migration extent relative to the filter paper. In both cementitious wasteforms, the migration extent increased in the order 152 Eu< 133 Ba< 60 Co< 137 Cs. However, less migration was measured when the radionuclides were incorporated into a reducing grout wasteform. The novelty of this paper is the demonstration of a technique capable of creating non-destructive measurements over decade time scales. Ultimately, this work provides insight into the long-term migration of alkali, alkali earth, divalent transition metal, and trivalent actinide element isotopes.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2025

Comparison of measurement techniques and sorption of radium-226 in low and high salinity aqueous samples

Human activities have the potential to redistribute radium (Ra) in the marine environment in a manner that may necessitate monitoring or management of subsequent human or environmental exposures. There is therefore a need to identify accurate and accessible techniques for Ra measurement in high salinity samples and to describe the distribution of Ra in estuarine and marine environments, but most efforts in these areas have focused on low salinity matrices. In addition, rapid and reliable measurements are crucial for time-sensitive samples such as short-lived isotopes or emergency situations. The objective of this study is to describe the limits of detection, cost, and relative ease for measurement of Ra in both low and high salinity aqueous samples via three analytical methods: liquid scintillation counting (LSC), high purity germanium (HPGe) gamma spectrometry, and inductively coupled plasma mass spectrometry (ICP-MS). To contextualize these measurements for real-world scenarios, the partitioning of 226 Ra to substrates relevant to the marine environment was also characterized. Although HPGe detection with solid phase extraction had the lowest limit of detection for low salinity samples (0.27 Bq L −1 ), poor 226 Ra recovery for high salinity samples and high materials costs make this method prohibitive for many users. Limits of detection for high salinity samples were lower for LSC (1.28 Bq L −1 ) than for ICP-MS without dilution (11.4 Bq L −1 ), but significant and unexpected degradation of the high salinity LSC standards was observed after six months. Furthermore, our preferred measurement method for high salinity Ra samples is ICP-MS with sample dilution as necessary to reduce matrix effects.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2026

Irradiation Impact on Uranium Recovery Under Direct Extraction Conditions

Reducing the quantity of high-level radioactive waste is essential for minimizing environmental impact and improving efficiency of using natural resources for nuclear power. The current standard, Plutonium Uranium Solvent EXtraction (PUREX), uses tributyl phosphate (TBP) ligands to extract complexes of uranium and plutonium from a nitric acid (HNO3) phase. Although this method is effective, large volumes of HNO3 and the non-incinerable phosphate ligands increase the amount of hazardous waste produced. Alternative extractants and flowsheets have been proposed that allow for more selective extraction of radioactive metals, reduced nitric acid use, and easier incineration by only containing carbon, hydrogen, oxygen, and nitrogen (CHON). One candidate, N,N-di(2-ethylhexyl)-isobutyramide (DEHiBA) exhibits promising properties for direct extraction. A HNO3 pre-equilibrated DEHiBA phase selectively extracts U(VI), leaving plutonium, transuranics, and fission products behind as precipitate and reducing the volume of radioactive HNO3 produced.

38 - RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCL↗
DOE OSTI2024

Radioactive Waste Management Basis (Rev.6)

This Radioactive Waste Management Basis (RWMB) documents radioactive waste management practices adopted at Lawrence Livermore National Laboratory (LLNL) pursuant to Department of Energy Order (DOE O) 435.1, Radioactive Waste Management. The purpose of this RWMB is to ensure that LLNL manages radioactive waste in a safe and environmentally-compliant manner, protective of worker and public safety.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2021

Annual Status Report (FY 2020): Performance Assessment for the Environmental Restoration Disposal Facility

DOE O 435.1 and DOE M 435.1-1 require that a determination of continued adequacy of the performance assessment (PA) (CP-60089), composite analysis, and disposal authorization statement (DAS) be made annually, and these guidelines must be used to consider the results of data collection and analysis from research, field studies, and monitoring as well as provide the need to update any radioactive waste management basis documents. Beginning in 1996, the Environmental Restoration Disposal Facility (ERDF) started accepting low-level radioactive, hazardous, and mixed wastes generated during cleanup activities at the Hanford Site. ERDF is composed of a series of cells or disposal areas and can accommodate future design expansions as needed. Currently, there are 10 cells. During this reporting period (fiscal year 2020, which extended from October 1, 2019, through September 30, 2020), approximately 3.39E+04 U.S. tons (3.07E+04 metric tons) of waste was disposed at ERDF. From ERDF inception through September 30, 2020, approximately 18.5 million U.S. tons of waste has been disposed at ERDF, which equates to the consumption of approximately 88% of the disposal volume. As a condition of the DAS, disposal operations within ERDF must be in accordance with the waste acceptance criteria (ERDF-00011) that provide specific radionuclide disposal limits, waste form restrictions, and descriptions of acceptable waste packages in compliance with DOE M 435.1-1 requirements. The ERDF waste acceptance criteria stipulate that waste destined for disposal at ERDF be controlled based on source, physical form, and contaminant concentration and activity levels. There have been no changes to the physical configuration of ERDF or to the waste forms (source, physical form, etc.). No new Unreviewed Disposal Question Screenings or Evaluations have been generated during this reporting period. Therefore, there are no noted impacts to the PA, composite analysis, DAS, or radioactive waste management basis documents resulting from the evaluations and screenings. Sum of fraction analysis shows that the disposed inventory meets both the concentration and inventory threshold requirements. A sum of fractions value is computed for ERDF sensitive radionuclides contributing to the all pathways and air pathway inventory limits. Computed values were 8.85E-02 and 1.78E-01, respectively. The disposed waste inventory remained well under the PA imposed limits. Required monitoring was satisfactorily completed during the fiscal year reporting period (fiscal year 2020). Compliance with performance objectives were met as each of the reported values were well below the established limit. Overall, there are no substantive changes to primary PA assumptions nor changes to the PA analysis conclusion; therefore, compliance with DOE O 435.1 and the DAS is maintained.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2025

Summary of Analytical Services for the Hanford Site Radionuclide NESHAP Program

This document is a summary of the point source analytical requirements used to demonstrate compliance for the Department of Energy (DOE) Hanford Site operations with 40 Code of Federal Regulations (CFR) Part 61, “National Emission Standards for Hazardous Air Pollutants,” (NESHAP) Subpart H, “National Emission Standards for Emissions of Radionuclides Other Than Radon From Department of Energy Facilities,” and the Washington Administrative Code (WAC) 246-247, “Radiation Protection – Air Emissions.” This reference collects information from multiple source documents and is not intended to create, supersede, replace or over-ride any existing contractual, DOE, federal or state statutes, regulations, compliance agreements, orders, permits, licenses or other requirements. The requirement source document governs where any difference may exist. The Hanford Mission Integration Solutions (HMIS) Environmental organization has been contracted by DOE to manage and report data collected from the sampling and monitoring of radioactive air emissions point sources, colloquially called stacks. The Environmental organization coordinates the analyses and reporting of samples collected at various facilities across the Hanford Site. These facilities operate approximately 52 stacks that require sampling, monitoring or estimating radioactive air emissions. The stacks are operated by Bechtel National, Inc. (BNI), Central Plateau Cleanup Company (CPCCo), Hanford Tank Waste Operations & Closure (H2C), Hanford Laboratory Management and Integration (HLMI), and Pacific Northwest National Laboratory (PNNL). Stack samples from CPCCo, HLMI and H2C facilities are collected by the operating contractor staff, delivered to HMIS, and then shipped to an offsite contracted laboratory for analyses. The field and laboratory sample data uploaded into the Sample Management and Analytical Results Tracking (SMART) database are used to calculate sample volumes and concentrations. Sample concentrations are evaluated for compliance with federal and state regulations, permits, and license requirements. The SMART database also calculates total curies released for sampled point sources and stacks. Point source effluent concentrations and releases are published annually in publicly available reports. The BNI and PNNL operate several DOE-Hanford Field Office (HFO) stacks subject to the requirements of 40 CFR 61, Subpart H and WAC 246-247. The concentrations, curies released and dose modeling evaluation for these stacks are included in the DOE-HFO annual radionuclide NESHAP report. The sample collection, analyses and emissions estimates for these stacks are outside the scope of HMIS contracted responsibilities and not addressed further in this document.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Environmental Air Monitoring at LANL: 2023 External Program Assessment [Slides]

Radioactive Air Emissions Management evaluates radiological impacts of LANL operations on members of the public, identifies and quantifies releases, and assesses impacts. It is not directly affiliated with cleanup operations or programmatic work and has independent oversight. The focus areas in Environmental Compliance Programs are stack emissions measurements, ambient air measurements, minor source operations evaluations, data management and quality assurance, collaboration with Meteorology program, and collaboration with Dose Assessment program (EPC-ES).

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Determining Unabated Airborne Radionuclide Emissions Monitoring Requirements Using Inventory-Based Methods

Compliance with the airborne radionuclide emission monitoring requirements in the National Emission Standards for Hazardous Air Pollutants (NESHAP; Title 40 of the U.S. Code of Federal Regulations Part 61, Subpart H) and State requirements in Washington Administrative Code 246–247: Radiation Protection – Air Emissions and 173-480: Ambient Air Quality Standards and Emission Limits for Radionuclides were evaluated for Pacific Northwest National Laboratory (PNNL) operations. Additional guidance may be found in the U.S. Department of Energy Handbook, Environmental Radiological Effluent Monitoring and Environmental Surveillance. To meet regulatory requirements, reviews of planned or proposed projects and activities provide the basis for implementing necessary monitoring adjustments or for implementing changes to projects and activities in a timely manner. Potential unabated off-site doses were evaluated for emission locations managed by PNNL and licensed to the Department of Energy. These locations were at facilities in Richland, Washington (i.e., the Hanford Site and PNNL–Richland campus) and in Sequim, Washington, (PNNL–Sequim campus). This report describes the inventory-based methods and provides the results for the NESHAP assessment performed in January 2024 for calendar year ending 2023.

40 CFR 61 Subpart H↗
DOE OSTI2025

Benchmark Exercise Report for Experimental Study of Bubble Scrubbing in Sodium Pool

Mechanistic source term (MST) analyses are likely to be an important part of advanced reactor licensing applications. For the purpose, an MST analysis code applicable to newly introduced advanced reactors, called SRT (Simplified Radionuclide Transport) code, has been developed by Argonne National Laboratory. SRT can track overall behaviors of radionuclides especially in metal fuel-based sodium fast reactors (SFRs) and microreactors. Throughout the simulation, migration inside fuel pins before failure, interaction with coolant (for SFR), removal/leakage in cover gas and containment (or confinement), and environmental dose impacts are considered alongside radioactive decay for short-lived nuclides. Among the postulated process, pool scrubbing phenomenon, especially under sodium pool condition, has been identified as high importance with limited supportive data. The phenomenon plays a crucial role in assessing the degree of radiological impacts as radioactive aerosols or vapors are efficiently and effectively removed during the process. To provide validation basis for SRT in assessing pool scrubbing performance inside sodium pools, the University of Wisconsin-Madison performed tests including extensive parametric effects. Separate effect tests were conducted to directly evaluate the SRT models and to estimate degree of contribution by each contributing factor. Specifically, bubble size, aerosol size, aerosol density, aerosol concentration, pool depth, system temperature, and bubble swarm effects were considered. According to the parametric effects, decontamination performance enhances with decreasing bubble size, large density, and deeper pool height. Aerosol concentration provides no effect for the whole range of interest, and pool temperature variation shows minor effects under the considered temperature condition. When multiple bubbles are injected generating a bubble swarm condition, DF performance further enhances by bubble interactions and turbulence characteristics. The measurement shows the exceptional importance of aerosol size range considered, with the lowest decontamination, where most radionuclides are expected to escape.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2023

Performance Assessment for the Environmental Restoration Disposal Facility (Annual Status Report FY 2022)

DOE O 435.1 and DOE M 435.1-1 require that a determination of continued adequacy of the performance assessment (PA) (CP-60089), composite analysis (CA), and disposal authorization statement (DAS) be made on an annual basis, and that the determination must consider the results of data collection and analysis from research, field studies, and monitoring as well as the need to update any Radioactive Waste Management Basis (RWMB) documents. Beginning in 1996, the Environmental Restoration Disposal Facility (ERDF) started accepting low-level radioactive, hazardous, and mixed wastes that were generated during cleanup activities at the Hanford Site. ERDF is composed of a series of cells or disposal areas and can accommodate future design expansions as needed. Currently, there are eight cells and two supercells in ERDF. Each supercell is the equivalent of two cells. During this reporting period (fiscal year 2022, extending from October 1, 2021, through September 30, 2022), approximately 8.52E+04 metric tons (9.39E+04 U.S. tons) of waste was disposed at ERDF. From ERDF inception through September 30, 2022, approximately 17.0 million metric tons (18.7 million U.S. tons) of waste has been disposed at ERDF, which equates to consumption of approximately 89.1% of the currently constructed disposal volume. According to the design of ERDF, the facility has the ability to be expanded as needed. As a condition of the DAS, disposal operations within ERDF must be in accordance with the waste acceptance criteria (ERDF-00011) that provide specific radionuclide disposal limits, waste form restrictions, and descriptions of acceptable waste packages in compliance with the requirements of DOE M 435-1.1. The ERDF waste acceptance criteria stipulate that waste destined for disposal at ERDF be controlled based on source, physical form, and contaminant concentration and activity levels. There have been no changes to the physical configuration of ERDF or to the waste forms (source, physical form, etc.). No new unreviewed disposal question screenings or evaluations have been generated in this reporting period. Therefore, there are no noted impacts to the PA, CA, DAS, or RWMB resulting from the evaluations and screenings. Sum-of-fractions analysis shows that the disposed inventory meets both the concentration and inventory threshold requirements. A sum-of-fractions value is computed for ERDF sensitive radionuclides contributing to the groundwater pathways and the air pathway inventory limits. Computed values were 5.50E-04 and 3.30E-03, respectively. The disposed waste inventory remained well under the PA imposed limits, as shown in Table 4 and Table 5 in the main text of this report. Required monitoring was satisfactorily completed during the fiscal year reporting period. Compliance with performance objectives were met as each of the reported values were well below the established limit. Overall, there are no substantive changes to primary PA assumptions or changes to the PA analysis conclusion; therefore, compliance with DOE O 435.1 and the DAS is maintained.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Using the CAP88 Plume Model & Dose Assessment Code for the FTWC Project

The Environmental Protection & Compliance Division (EPC) uses the Clean Air Act Assessment Package – 1988 (CAP88) plume model and dose assessment code to evaluate measured emissions or projected emissions of airborne radionuclides from Los Alamos National Laboratory (LANL) facilities. This software package will use facility data (e.g., stack height and exit velocity), emissions parameters (chemical form and quantity), and environmental data (wind speed and direction) to predict downwind concentrations of radioactive material and subsequent dose to a member of the public at that location. The United States Environmental Protection Agency (EPA) has approved CAP88 for use in demonstrating compliance with the Radionuclide NESHAP2, that portion of the Clean Air Act addressing emissions of airborne radioactive material from Department of Energy facilities. EPC Division has two procedures which discuss the use of CAP88.

61 RADIATION PROTECTION AND DOSIMETRY↗
DOE OSTI2022

Performance Assessment for the Environmental Restoration Disposal Facility (Annual Status Report FY 2021)

DOE O 435.1 and DOE M 435.1-1 require that a determination of continued adequacy of the performance assessment (PA) (CP-60089), composite analysis (CA), and disposal authorization statement (DAS) be made on an annual basis, and that the determination must consider the results of data collection and analysis from research, field studies, and monitoring as well as the need to update any Radioactive Waste Management Basis (RWMB) documents. Beginning in 1996, the Environmental Disposal Facility (ERDF) started accepting low-level radioactive, hazardous, and mixed wastes that were generated during cleanup activities at the Hanford Site. ERDF is composed of a series of cells or disposal areas and can accommodate future design expansions as needed. Currently, there are eight cells and two supercells in ERDF. Each supercell is the equivalent of two cells. During this reporting period (fiscal year 2021, extending from October 1, 2020, through September 30, 2021), approximately 9.14E+04 metric tons (1.01E+05 U.S. tons) of waste was disposed at ERDF. From ERDF inception through September 30, 2021, approximately 16.9 million metric tons (18.9 U.S. tons) of waste has been disposed of at ERDF, which equates to consumption of approximately 88.7% of the currently constructed disposal volume. According to the design of ERDF, the facility has the ability to be expanded as needed. As a condition of the DAS, disposal operation within ERDF must be in accordance with the waste acceptance criteria (ERDF-00011) that provide specific radionuclide disposal limits, waste form restrictions, and descriptions of acceptable waste packages in compliance with the requirements of DOE M 435-1.1. The ERDF waste acceptance criteria stipulate that waste destined for disposal at ERDF be controlled based on source, physical form, and contaminant concentration and activity levels. There have been no changes to the physical configuration of ERDF or to the waste forms (source, physical form, etc.). No new unreviewed disposal question screenings or evaluations have been generated in this reporting period. Therefore, there are no noted impacts to the PA, CA, DAS, or RWMB resulting from the evaluations and screenings. Sum-of-fractions analysis shows that the disposed inventory meets both the concentration and inventory threshold requirements. A sum-of-fractions value is computed for ERDF sensitive radionuclides contributing to the all pathways and the air pathway inventory limits. Computed values were 7.63E-03 and 1.49E-03, respectively. The disposed waste inventory remained well under the PA imposed limits, as shown in Table 4 and Table 5 in the main text of this report. Required monitoring was satisfactorily completed during the fiscal year reporting period. Compliance with performance objectives were met as each of the reported values were well below the established limit. Overall, there are no substantive changes to primary PA assumptions or changes to the PA analysis conclusion; therefore, compliance with DOE O 435.1 and the DAS is maintained.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2023

129 I, 99 Tc, And U Distribution Coefficients of Subsurface Sediments Collected from the Proposed Site of the Environmental Management Disposal Facility

Performance Assessment calculations were completed in 2020 to evaluate the Environmental Management Disposal Facility (EMDF), a proposed new low-level radioactive waste (LLW) disposal facility on the U.S. Department of Energy’s Oak Ridge Reservation (ORR). Among the large number of input parameters needed for such calculations, are distribution coefficients (K d values; radionuclide concentration solid:liquid ratio) that provide a measure of the tendency of radionuclides to bind to sediments. The objective of this study was to measure K d values of three radionuclides that may pose a disproportionately large amount of risk, U, 129 I and 99 Tc. The average I K d value for the 14 geological materials recovered from the proposed EMDF site was 37.8 mL/g and ranged from -1.8 to 140.9 mL/g. These values were consistent, but somewhat larger than previous measurements made with ORR sediments and were about an order of magnitude greater than those used in previous EMDF PA calculations. The median Tc K d value was 365.7 mL/g, much greater than previously reported using ORR geological materials. Five of the 14 tested geological materials sorbed large quantities of Tc, suggesting that the weakly sorbing Tc(VII) species had been reduced to the sparingly soluble Tc(IV) species. The five strongly sorbing sediments had apparent Tc solubility values of approximately <10 -8 mol/L. The median U K d value was 5,726 mL/g. All of the tested geological materials had large K d values, ranging from 625 to >10,208 mL/g. Among the sediment samples that exhibited strong U binding, the apparent solubility value was approximately <10 -9 mol/L. Based on sediment properties and general ORR geological considerations, it was proposed that much of the I and Tc retention could be attributed to the site materials exhibiting low pH (average pH = 4.94), low redox status, and/or the elevated levels of iron oxides, manganese oxides, and natural organic matter. Similarly, the extremely high U binding measured in these sediments may also be attributed to the low conditions of carbonates, which can complex and therefore solubilize uranyl in these tests due to the low pH, and also the relatively high concentrations of iron and organic coatings on these samples. An implication of this study is that the areas of the EMDF subsurface environment may have natural properties for attenuating I, Tc, and U movement, and potentially other radionuclides, thereby possibly reducing risk posed by burial of LLW at this site. This document is a revision of SRNL-STI-2021-00404, Revision 0 that includes new data describing U K d values and new I and Tc K d values for four Nolichucky sediments. These new results were integrated into the data presented in the original document.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2025

129 I, 99 Tc, and U Distribution Coefficients of Subsurface Sediments Collected from the Proposed Site of the Environmental Management Disposal Facility

Performance Assessment calculations were completed in 2020 to evaluate the Environmental Management Disposal Facility (EMDF), a proposed new low-level radioactive waste (LLW) disposal facility on the U.S. Department of Energy’s Oak Ridge Reservation (ORR). Among the large number of input parameters needed for such calculations, are distribution coefficients (K d values; radionuclide concentration solid: liquid ratio) that provide a measure of the tendency of radionuclides to bind to sediments. The objective of this study was to measure K d values of three radionuclides that may pose a disproportionately large amount of risk, U, iodine-129 ( 129 I) and technetium-99 ( 99 Tc). The average 129 I K d value for the 14 geological materials recovered from the proposed EMDF site was 37.8 mL/g and ranged from 0.45 to 140.9 mL/g. These values were consistent, but somewhat larger than previous measurements made with ORR sediments and were about an order of magnitude greater than those used in previous EMDF PA calculations. The median 99 Tc K d value was 365.7 mL/g, much greater than previously reported using ORR geological materials. Five of the 14 tested geological materials sorbed large quantities of 99 Tc, suggesting that the weakly sorbing 99 Tc(VII) species had been reduced to the sparingly soluble 99 Tc(IV) species. The five strongly sorbing sediments had apparent 99 Tc solubility values of approximately <10 -8 mol/L. The median U K d value was 5,726 mL/g. All of the tested geological materials had large K d values, ranging from 625 to >10,208 mL/g. Among the sediment samples that exhibited strong U binding, the apparent solubility value was approximately <10 -9 mol/L. Based on sediment properties and general ORR geological considerations, it was proposed that much of the 129 I and 99 Tc retention could be attributed to the site materials exhibiting low pH (average pH = 4.94), and/or the elevated levels of iron oxides, manganese oxides, and natural organic matter. Similarly, the extremely high U binding measured in these sediments may also be attributed to the low conditions of carbonates, which can complex and therefore solubilize uranyl in these tests due to the low pH, and also the relatively high concentrations of iron and organic coatings on these samples. An implication of this study is that the areas of the EMDF subsurface environment may have natural properties for attenuating 129 I, 99 Tc, and U movement, and potentially other radionuclides, thereby possibly reducing risk posed by burial of LLW at this site.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗